Influence of SO2 in incineration flue gas on the sequestration of CO2 by municipal solid waste incinerator fly ash

The influence of CO2 content and presence of SO2 on the sequestration of CO2 by municipal solid waste incinerator(MSWI) fly ash was studied by investigating the carbonation reaction of MSWI fly ash with different combinations of simulated flue gas.The reaction between fly ash and 100% CO2 was relatively fast;the uptake of CO2 reached 87g CO2/kg ash,and the sequestered CO2 could be entirely released at high temperatures.When CO2 content was reduced to 12%,the reaction rate decreased;the uptake fell to 41g CO2/kg ash,and 70.7% of the sequestered CO2 could be released.With 12% CO2 in the presence of SO2,the reaction rate significantly decreased;the uptake was just 17g CO2/kg ash,and only 52.9% of the sequestered CO2 could be released.SO2 in the simulated gas restricted the ability of fly ash to sequester CO2 because it blocked the pores of the ash.     

TiO2-Fe3+可见光催化H2O2降解阿特拉津的协同效应

以内分泌干扰物阿特拉津为模型污染物,研究了TiO2-Fe3+可见光催化H2O2降解阿特拉津的协同效应.结果表明,在H2O2存在条件下,金红石TiO2经可见光激发可持续稳定地产生.OH自由基,在Fe3+协同作用下,.OH自由基生成量急剧增加;TiO2能可见光催化H2O2降解阿特拉津,金红石TiO2显示出较锐钛矿TiO2及混晶TiO2(TiO2P25)更高的催化活性,反应60 min,阿特拉津的降解率可达40%;以Fe3+协同TiO2可见光催化H2O2降解阿特拉津时,反应效率显著加快,反应5 min即对阿特拉津的降解率达到100%,而金红石TiO2显示出更为明显的协同效应.     

Studies on the formation of H2O2 in the ozonolysis of alkenes

The formation of H₂O₂ in the reactions of ozone with alkenes, isoprene and some terpenes has been studied with tunable diode laser absorption spectroscopy. The measured yields of H₂O₂ were found to be considerably enhanced in the presence of water vapour. H₂O₂ is thought to be formed in the ozonolysis of the alkene with O₃ by direct reaction of an intermediate with water vapour. The yield of H₂O₂ relative to the reacted alkene in the ozonolysis of trans-2-butene in the presence of water vapour was also studied with long path FTIR spectroscopy. Irrespective of the analytical methods and reaction conditions applied, the H₂O₂ yields in the reaction of O₃ with the different alkenes in the presence of water vapour were found to be in the range of a few per cent or less. Under the assumption that the reactive species forming H₂O₂ in the ozonolysis is the Criegee biradical, the overall rate constants for the reactions of some biradicals with water vapour were measured relative to the rate constant of the biradical with SO₂. For the H₂COO biradical a rate constant of (5.8 ± 2.5) × 10⁻¹⁷ cm³ s⁻¹ was determined and for the (CH₃)₂COO biradical (2.9 ± 1.5) × 10⁻¹⁷ cm³ s⁻¹; in the latter case with the assumption that (CH₃)₂COO reacts with SO₂ as fast as CH₂COO.     

环境污染物浓缩铀诱发雄性机体的生殖毒性研究

在不同水平浓缩铀￣（２３５）ＵＯ＿２Ｆ＿２内污染诱发机体生殖毒性的研究中，观察到浓缩铀可诱发精子畸形，主要呈现双头和无钩精子。浓缩铀诱发精原细胞染色体畸变，则以染色体断片为主，对初级精母细胞可产生染色体断片和易位，出现多价体。浓缩铀可致精子ＤＮＡ链断裂，其断裂片段则可随￣（２３５）ＵＯ＿２Ｆ＿２摄入量的加大而增多，浓缩铀引起遗传物质的损伤，可诱发胎鼠显性致死突变和骨骼畸形增生，而其诱发骨骼畸形的发生率则与睾丸浓缩铀的摄入量呈正相关。     

Some aqueous reactions of potential importance in the atmospheric chemistry of mercury

Reactions of Hg(I) and Hg(II) with oxidizing and reducing agents have been investigated using stopped-flow and spectroscopic techniques. Hg₂²⁺ was found to be oxidized by HClO and radicals produced by Fentons reagent (Fe²⁺ + H₂O₂). The rate determining step in the reaction of Hg₂²⁺ and HClO is probably a relatively rapid reaction of Hg⁰ and HClO. A photochemically induced reduction of Hg(OH)₂(aq) to Hg⁰ was observed when irradiating with simulated sunlight (λ>290 nm), which may be a process of environmental importance. Aqueous Hg(CN)₂ and HgCl₂ were found to be stable. The rate of reduction of Hg(SO₃)₂²⁻ is not affected by irradiation. No oxidation of Hg₂²⁺ was found when mixing solutions containing H₂O₂ or Fe³⁺ or a mixture of the two which suggests that H₂O₂ is not an important oxidant for mercury under environmental conditions.     

Quantification of nitro- and hydroxylated nitro-aromatic/polycyclic aromatic hydrocarbons in selected ambient air daytime winter samples

Two ambient air samples, both collected in a northern latitude city during winter daytimes, are compared here with regard to NO₂-AR/PAH levels and OH-NO₂-AR levelsfrom filter and XAD-2 extracts. Detection of a previously unreported environmental constituent, tentatively identified as a NO₂-azulene isomer, is discussed. The levels of the OH-NO₂-AR were, in general, at least 4 times higher than levels of the corresponding NO₂-AR. As with NO₂-AR/PAH, OH-NO₂-AR appear to be both primary source emissions and secondary photochemical products. The filter-collected para-substituted OH-NO₂-AR in these samples appear to be the source emissions, while the XAD-collected ortho- and para-substituted OH-NO₂-AR may be products of photochemical reactions. Other pollutant and meteorological data, including NO, NO₂, HONO, sunlight intensity and fine-particle Pb and K concentrations, are also used to discuss differences between these samples.     

培养基中磷酸盐在GA1所产絮凝剂絮凝中的作用研究

考察了一株高效产絮凝剂微生物多粘类芽孢杆菌Paenibacillus polymyxa GA1(以下简称GA1)的发酵培养基以及培养基各组分的絮凝性.实验结果表明,培养基中K2HPO4、KH2PO4在CaCl2存在、pH值中性偏碱时对各种废水均有一定的絮凝性,在GA1所产絮凝剂(以下简称MBFGA1)絮凝废水的过程中起重要作用,且作用离子为PO43-和Ca2 ;这两种离子在pH值中性偏碱时能有效降低高岭土悬液的ζ电位绝对值到接近零,使胶体脱稳;PO43-和Ca2 形成絮状沉淀后,能网捕脱稳颗粒,进而在MBFGA1桥联作用下使颗粒结团沉降完成絮凝.发酵培养基虽有一定絮凝性,但效果不佳,处理后上清液颗粒平均粒径远大于发酵液处理,且絮体、泥饼性质差异大,不利于工业应用和后续处理.硫酸钡亦有一定的助凝效果,但因沉淀本身性质差异,其效果劣于磷酸钙.     

污水处理过程N2O排放：过程机制与控制策略

污水处理生物脱氮过程中氧化亚氮(N₂O)作为直接碳排放源,其大气升温效应较CO₂高出265倍.因此,国际上对N₂O排放机制与控制策略的研究层出不穷.N₂O产生源于硝化与反硝化过程,主要涉及亚硝化(AOB)及其同步反硝化、常规异养反硝化(HDN)、同步异养硝化-好氧反硝化(HN-AD)和全程氨氧化(COMAMMOX)等生物途径,以及硝化过程中间产物NH₂OH与NOH之非生物化学途径.常规硝化与反硝化(AOB+HDN)途径在正常运行工况下N₂O排放量并不是很大,约只占进水TN负荷的1.3%;即使是HN-AD与COMAMMOX代谢过程,两者N₂O产生量也不足TN负荷的0.5%.不可忽视的是AOB亚硝化及其同步反硝化,它们已被确认为是污水处理生物脱氮过程中N₂O排放的首要途径;AOB过程中间产物(NH₂OH与NOH)非生物化学过程以及AOB反硝化生物过程(主途径)共同导致的N₂...     

Deep Geological CO2 Storage: Principles Reviewed, and Prospecting for Bio-energy Disposal Sites

The principles of hydrocarbon exploration and production provide well-established and tested principles and technologies to investigate storage of fluids in the subsurface. CO₂ can be stored in the subsurface using settings of: (A) thick permeable coal seams; (B) depleted oil and gas fields; (C) saline aquifers of regional extent, with an overlying seal. The North Sea Sleipner project shows that CO₂ can be injected into the pore space of deep geological aquifers deeper than 800 m at 1 Mt/yr, using established technology. Suitable sediment sequences of saline aquifers exist in all hydrocarbon-producing areas, are volumetrically much larger than exploited oil and gas fields, and hold the potential to easily store all worldwide CO₂ emissions until 2050. Geological principles are established to assess entire continents for candidate sites of CO₂ storage. This shows that opportunity may be widespread, but needs more specific local investigations. Onshore sub-Saharan Africa is considered the most problematic region – but even here there are potentially viable sediment sequences. No demonstration projects currently exist for CO₂ capture and storage using small-scale onshore facilities. A simple estimate, assuming CO₂ value of $20 per ton, suggests that single boreholes onshore may be viable over 20 years with supply rates of 100,000 ton CO₂ per year. In principle, atmospheric CO₂ could be captured by cultivated biomass, and co-fired in existing power stations. Or energy crops could be grown, CO₂ to be used, and stored deep below ground, in a country distant from an original fossil-fuel CO₂ emission site.     

基于碳捕集的富氧燃煤烟气联合脱硫脱硝试验研究

富氧燃煤烟气压缩液化CO2的高压低温工况为NO氧化为易溶于水的NO2提供了十分有利的条件.基于小型高压吸收试验装置,采用配制的富氧燃煤模拟烟气,在高压常温下进行了NO、SO2、O2与H2O的吸收反应试验.根据反应前后的气液产物分析,测定了不同组分比例与不同压力下混合气体中NO与SO2的转化率.NO氧化与吸收试验表明,NO转化为HNO3的比率随压力升高而增加,在0.5 ～2 MPa之间增加很快,在2 ～3 MPa之间增速趋丁平缓,压力达3 MPa以上时,90％以上的NO均转化为稀硝酸,且初始NO浓度越高,NO的转化率越大.混合气体中同时存在5O2与NO的联合吸收试验发现,只有少量的NO转化成了NO3-,SO2向H2SO4的转化率随压力升高而增加,初始SO2浓度越大,转化率越高.分析表明,SO2与NO同时存在时SO2先行转化为SO3,NO充当了催化剂,但SO2转化为SO3的一次转化率小于35％,反应酸液产物的多次循环能使SO2的转化率达到90％以上.建议的工艺流程中需采用两座吸收反应塔顺序脱除SO2与NO并回收稀酸溶液,有望在富氧燃煤发电捕集CO2系统中降低脱硫脱硝成本,部分地弥补富氧燃烧机组发电成本的增加.     

深部储层中CO2沿断层泄漏量的影响因素

CGS（CO₂地质储存）是CO₂减排的重要手段之一,天然裂隙的存在则是CGS的潜在风险.CO₂地质储存过程中储层上覆盖层及其浅部含水层是防止CO₂泄漏的天然屏障,为了探究深部咸水层中CO₂沿断层的泄漏过程并获得断层渗透率及储层中超临界CO₂流体初始条件（初始饱和度、初始泄漏压力）对CO₂沿断层泄漏速率和泄漏量的影响程度,依据鄂尔多斯CO₂灌注工程示范区资料,使用多相、多组分溶质运移数值模拟软件TOUGH2建立了2D概念模型.结果表明,深部咸水层中的CO₂在压力差和浓度差的作用下沿断层发生泄漏,到达浅部含水层后开始发生侧向运移,100 a内运移了约200 m的水平距离;由于浮力的作用,CO₂集中在含水层顶板处,有效地防止了CO₂向外泄漏.影响因素分析表明,100 a内断层渗透性能为低渗、中渗和高渗条件时,CO₂累积泄漏量分别为0、1 050和3 000 t;CO₂初始饱和度分别为0.20、0.50和0.99时,CO₂累积泄漏量分别为550、1 050和1 650 t;初始泄漏压力分别为17.3、17.6和18.1 MPa时,CO₂累积泄漏量则分别为900、1 050和1 400 t.除此之外,断层渗透性、CO₂初始气体饱和度和初始泄漏压力对CO₂泄漏的影响还体现在泄漏发生时间和平均泄漏速率上.研究显示,各因素对CO₂沿断层泄漏过程的影响程度表现为断层渗透性能> CO₂初始饱和度> CO₂初始泄漏压力.      

An estimate of the conversion rates of SO2 to SO2-4 and NO2 to HNO3+ NO3- for the evaluation air pollution in Beijing

The conversion rates of SO₂ to SO^2-₄ and NO₂ to HNO₃₊NO₃- are estimated from the field-data obtained in Beijing in summer, 1988. The results show that the conversion rate of NO₂ is about four times as much as that of SO₂; The conversion rates have a diurnal variation in a day. On the average, the rate of SO₂ is estimated to be 4.7% h^-1 during the daytime and 3.4% h^-1 during the nighttime. Similarly, the rate of NO₂ is estimated to be 17.2% h^-1 and 12% h^-1 respectively.     

Numerical evaluation of the effectiveness of NO2 and N2O5 generation during the NO ozonation process

Wet scrubbing combined with ozone oxidation has become a promising technology for simultaneous removal of SO₂ and NO_x in exhaust gas. In this paper, a new 20-species, 76-step detailed kinetic mechanism was proposed between O₃ and NO_x. The concentration of N₂O₅ was measured using an in-situ IR spectrometer. The numerical evaluation results kept good pace with both the public experiment results and our experiment results. Key reaction parameters for the generation of NO₂ and N₂O₅ during the NO ozonation process were investigated by a numerical simulation method. The effect of temperature on producing NO₂ was found to be negligible. To produce NO₂, the optimal residence time was 1.25 sec and the molar ratio of O₃/NO about 1. For the generation of N₂O₅, the residence time should be about 8 sec while the temperature of the exhaust gas should be strictly controlled and the molar ratio of O₃/NO about 1.75. This study provided detailed investigations on the reaction parameters of ozonation of NO_x by a numerical simulation method, and the results obtained should be helpful for the design and optimization of ozone oxidation combined with the wet flue gas desulfurization methods (WFGD) method for the removal of NO_x.     

Reaction of monoterpenes with ozone,sulphur dioxide and nitrogen dioxide—gas-phase oxidation of SO2 and formation of sulphuric acid

Teflon bag experiments were carried out in the dark in order to study the gas-phase reactions of selected monoterpenes with O₃ in the presence of SO₂ (β-pinene) as well as in the presence of SO₂/NO₂ (α-pinene, β-pinene, limonene). Emphasis was given in identifying the main reaction products and in quantifying the H₂SO₄ aerosol formed. Apart from the H₂SO₄ aerosol no other S containing compounds could be detected.It was found that the reaction of β-pinene with O₃, SO₂ and NO₂ leads mainly to 6,6-dimethyl-bicyclo [3.1.1] heptan-2-one (nopinone), the α-pinene-O₃-SO₂-NO₂-reaction produced 2′,2′-dimethyl-3-acetyl cyclobutyl ethanal (pinonaldehyde). The reaction of limonene with O₃-SO₂-NO₂ leads mainly to an unidentified product with a molecular weight M⁺ 134. In addition to the above-mentioned volatile products, the formation of organic nitrates could be established by means of gas chromatography-mass spectrometry.The yield of H₂SO₄ in the system β-pinene/O₃/SO₂ varies between 0.13 and 0.44 depending on the initial conditions, e.g. humidity. In the system terpene/O₃/SO₂/NO₂ the yield of H₂SO₄ for α-pinene (after 1 h reaction time) was 0.01–0.03, for β-pinene (2 or 4 h reaction time) 0.07–0.13 and for limonene (1 h reaction time) 0.02–0.09.     

水蒸气电晕放电下的烟气脱硫效果

采用多针-板式电极,在70 m³/h烟气流量范围内,研究了水蒸气浓度、烟气流量、电场强度等因素对不饱和水蒸气正直流电晕放电烟气脱硫率的影响以及水蒸气电晕放电对脉冲放电烟气脱硫率的提高.研究结果表明,实验范围内,按照NH₃∶SO₂摩尔比为2∶1添加NH3的条件下,增加水蒸气流量、增强电场强度、减少烟气流量,烟气脱硫率能提高10%,达到60%左右.同时,水蒸气电晕放电能使脉冲放电的烟气脱硫率提高5%左右,达到90%以上.     

TiO2/Ti光电极电助光催化降解甲草胺的研究

采用阳极氧化法制备了TiO₂/Ti光电极,并通过电助光催化的方法研究了恒电流法和恒电压法对甲草胺的降解效率.实验证实了在光催化和电催化之间存在协同效应,反应溶液中加入Na₂SO₄电解质后,SO₄^2-可以被价带空穴氧化成强氧化性的S₂O₈^2-,继而可以氧化处理物质,提高甲草胺的降解效率.实验结果表明：甲草胺在羟基自由基的作用下通过羟基化作用和脱烷作用,发生断键、开环等一系列的氧化还原反应,最终生成CO₂和H₂O等无机小分子物质.     

Interactions of sulfuric acid with common atmospheric bases and organic acids: Thermodynamics and implications to new particle formation

Interactions of the three common atmospheric bases, dimethylamine ((CH₃)₂NH), methylamine (CH₃NH₂), ammonia (NH₃), all considered to be efficient stabilizers of binary clusters in the Earth's atmosphere, with H₂SO₄, the key atmospheric precursor, and 14 common atmospheric organic acids (COAs) (formic, acetic, oxalic, malonic, succinic, glutaric acid, adipic, benzoic, phenylacetic, pyruvic, maleic acid, malic, tartaric and pinonic acids) have been studied using the density functional theory (DFT) and composite high-accuracy G3MP2 method. The thermodynamic stability of mixed (COA)(H₂SO₄), (COA)(B1), (COA)(B2) and (COA)(B3) dimers and (COA)(H₂SO₄)(B1), (COA)(H₂SO₄)(B2) and (COA)(H₂SO₄)(B3) trimers, where B1, B2 and B3 refer to (CH₃)₂NH, CH₃NH₂ and NH₃, respectively, have been investigated and their impacts on the thermodynamic stability of clusters containing H₂SO₄ have been studied. Our investigation shows that interactions of H₂SO₄ with COA, (CH₃)₂NH, CH₃NH₂ and NH₃ lead to the formation of more stable mixed dimers and trimers than (H₂SO₄)₂ and (H₂SO₄)₂(base), respectively, and emphasize the importance of common organic species for early stages of atmospheric nucleation. We also show that although amines are generally confirmed to be more active than NH₃ as stabilizers of binary clusters, in some cases mixed trimers containing NH₃ are more stable thermodynamically than those containing CH₃NH₂. This study indicates an important role of COA, which coexist and interact with that H₂SO₄ and common atmospheric bases in the Earth atmosphere, in formation of stable pre-nucleation clusters and suggests that the impacts of COA on new particle formation (NPF) should be studied in further details.     

Photodegradation of amoxicillin by catalyzed Fe3+/H2O2 process

Three oxidation processes of UV-Fe³⁺(EDTA)/H₂O₂ (UV: ultraviolet light; EDTA: ethylenediaminetetraacetic acid), UV-Fe³⁺/H₂O₂ and Fe³⁺/H₂O₂ were simultaneously investigated for the degradation of amoxicillin at pH 7.0. The results indicated that, 100% amoxicillin degradation and 81.9% chemical oxygen demand (COD_Cr) removal could be achieved in the UV-Fe³⁺ (EDTA)/H₂O₂ process. The treatment efficiency of amoxicillin and COD_Cr removal were found to decrease to 59.0% and 43.0% in the UV-Fe³⁺/H₂O₂ process; 39.6% and 31.3% in the Fe³⁺/H₂O₂ process. Moreover, the results of biodegradability (biological oxygen demand (BOD₅)/COD_Cr ratio) revealed that the UV-Fe³⁺ (EDTA)/H₂O₂ process was a promising strategy to degrade amoxicillin as the biodegradability of the effluent was improved to 0.45, compared with the cases of UV-Fe³⁺/H₂O₂ (0.25) and Fe³⁺/H₂O₂ (0.10) processes. Therefore, it could be deduced that EDTA and UV light performed synergetic catalytic effect on the Fe³⁺/H₂O₂ process, enhancing the treatment efficiency. The degradation mechanisms were also investigated via UV-Vis spectra, and high performance liquid chromatography-mass spectra. The degradation pathway of amoxicillin was further proposed.     

程序升温条件下铁及其氧化物在CO存在时对N2O的还原机理

应用热综合分析仪（TG－FTIR）研究了在还原性气氛下Fe及其氧化物对N2O的催化还原 作用。研究发现铁氧化物对氮氧化物的催化还原能力相当弱，而Fe可以高效地降低N2O分解的初始温度和提高N2O向N2的转化率。在Fe和CO的作用下，N2O的初始分解温度为920K和1000K。在1123K时，N2O的转化率达到95％和805。TG／DSC曲线表明了在Fe与N2O反应过程中CO的作用表现为通过与N2O在反应表面的竞争吸附使铁氧化物还原为金属铁，X射线衍射证明Fe与N2O反应后的氧化物为Fe2O3；扫描电镜对反应后Fe表面物理形态的研究发展，在CO作用下，Fe的表面呈松散结构，可以保证Fe对氮氧化物反应的连续进行。     

MnFe2O4磁性纳米棒非均相Fenton催化降解水中四环素的研究

采用水热合成法成功制备出MnFe₂O₄磁性纳米棒(s-MnFe₂O₄),并考察了商品化的Fe₃O₄、MnFe₂O₄和合成的s-MnFe₂O₄纳米棒这3种磁性纳米颗粒作为非均相Fenton催化剂降解水中四环素抗生素的性能.同时,采用X射线衍射(XRD)、透射电镜(TEM)、N₂吸附-脱附、振动样品磁强计(VSM)及X射线光电子能谱(XPS)等技术对催化剂的理化性质进行了表征.非均相Fenton催化降解四环素的结果表明,s-MnFe₂O₄具有最高的催化活性,反应180 min,四环素的去除率可以达到87.6%,TOC的去除率达到47.5%.自由基捕获试验证实了羟基自由基(·OH)是非均相Fenton氧化过程中的主要活性物种.s-MnFe₂O₄磁性纳米棒的高催化活性归...